RT Journal Article T1 Silylation of lignin as an effective tool for the development of bio-based oil structuring materials A1 Trejo Cáceres, Manuel Ángel A1 Martín Alfonso, José Enrique A1 Franco Gómez, José María K1 Lignin; Silylation process; Bio-lubricant; Rheology; Friction and wear AB In this work, silylation process was employed as straightforward approach to develop biolubricants based on kraft lignin. The silylation reaction was conducted using tert-butyldimethylsilyl chloride (TBDMSCl) in the presence of dimethylformamide and imidazole as solvent and catalyst, respectively. By adjusting reaction times (2-24 h), several levels of physicochemical modification were achieved. Structural analysis via FTIR and two-dimensional 1H–13C HSQC NMR spectroscopy confirmed the successful incorporation of silane groups into lignin chemical structure, improving wettability and dispersibility. Additionally, SEM revealed notable changes in lignin particle morphology, particularly in particle size and aggregation. These physicochemically modulable amphipathic particles, containing hydrophilic groups and hydrophobic silane segments, were incorporated into castor oil and significantly impacted the rheological and tribological properties of the oleo-dispersions. Two distinct rheological behaviours were observed: liquid-like (at low reaction times <5 h) and gel-like (at high reaction times, > 16 h), where the silane groups, which act as a “bridge” for interaction with castor oil, and the area/volume ratio of lignin particles played a key role. The anti-friction and anti-wear properties were excellent, similar to or better than those obtained with castor oil or traditional lithium lubricating greases, attributed to the mending effect of the silylated lignin particles. This work offers a fast and straightforward compatibilization strategy to produce sustainable oil structuring agents, particularly relevant in the lubricant industry. PB Elsevier YR 2026 FD 2026 LK https://hdl.handle.net/10272/28125 UL https://hdl.handle.net/10272/28125 LA eng NO Trejo-Cáceres, M., Martín-Alfonso, J. E., & Franco, J. M. (2026). Silylation of lignin as an effective tool for the development of bio-based oil structuring materials. Polymer, 350, 129769. https://doi.org/10.1016/j.polymer.2026.129769 NO This work is part of the Research Projects PID2021-125637OB-I00 and PID2024-159052OB-I00, funded by MICIU/AEI/10.13039/501100011033 and by ERDF/EU and project Ref. 802C1800001, cofunded by ERDF/EU (80%) and Junta de Andalucía (Consejería de Economía, Conocimiento, Empresas y Universidades/Agencia-IDEA). Funding is gratefully acknowledged. Funding for open access charge: Universidad de Huelva/CBUA. DS Repositorio Institucional de la Universidad de Huelva RD 30 may 2026